The Effect of Heavy Ion Irradiation on the Forward Dissolution Rate of Borosilicate Glasses Studied In Situ and Real Time by Fluid-Cell Raman Spectroscopy

Autor: Mara Iris Lönartz, Lars Dohmen, Christoph Lenting, Christina Trautmann, Maik Lang, Thorsten Geisler
Jazyk: angličtina
Rok vydání: 2019
Předmět:
Zdroj: Materials, Vol 12, Iss 9, p 1480 (2019)
Druh dokumentu: article
ISSN: 1996-1944
12091480
DOI: 10.3390/ma12091480
Popis: Borosilicate glasses are the favored material for immobilization of high-level nuclear waste (HLW) from the reprocessing of spent fuel used in nuclear power plants. To assess the long-term stability of nuclear waste glasses, it is crucial to understand how self-irradiation affects the structural state of the glass and influences its dissolution behavior. In this study, we focus on the effect of heavy ion irradiation on the forward dissolution rate of a non-radioactive ternary borosilicate glass. To create extended radiation defects, the glass was subjected to heavy ion irradiation using 197Au ions that penetrated ~50 µm deep into the glass. The structural damage was characterized by Raman spectroscopy, revealing a significant depolymerization of the silicate and borate network in the irradiated glass and a reduction of the average boron coordination number. Real time, in situ fluid-cell Raman spectroscopic corrosion experiments were performed with the irradiated glass in a silica-undersaturated, 0.5 M NaHCO3 solution at temperatures between 80 and 85 °C (initial pH = 7.1). The time- and space-resolved in situ Raman data revealed a 3.7 ± 0.5 times increased forward dissolution rate for the irradiated glass compared to the non-irradiated glass, demonstrating a significant impact of irradiation-induced structural damage on the dissolution kinetics.
Databáze: Directory of Open Access Journals
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